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Estructura y reactividad de un complejo de nitrido de manganeso con un ligando tetramido macrocíclico
Huatian Shi1, Hung Kay Lee2, Yi Pan1
1Department of Chemistry, City University of Hong Kong, Tat Chee Avenue, Kowloon Tong, Hong Kong, China.
Journal of the American Chemical Society
|September 9, 2021
Resumen
Este estudio informa el aislamiento de un raro complejo de nitrido de manganeso, [MnVI Este complejo estable exhibe una reactividad única, actuando como electrófilo y nucleófilo en las reacciones de transferencia de átomos N e hidruro.
Área de la Ciencia:
- Química inorgánica
- Química organometálica
- Química del manganeso
Sus antecedentes:
- Los complejos de manganeso en el estado de oxidación +6 son excepcionalmente raros y típicamente inestables.
- Anteriormente, los complejos de nitrido de Mn (VI) se generaban en solución, pero eran demasiado inestables para su aislamiento.
Objetivo del estudio:
- Aislar y caracterizar un complejo estable de nitrido de manganeso.
- Investigar la reactividad del complejo de nitruro de Mn (VI) aislado en las reacciones de transferencia de átomos de N e hidruro.
- Para dilucidar el mecanismo de las reacciones de transferencia de hidrógeno con análogos de NADH.
Principales métodos:
- Oxidación de un electrón de un precursor de nitrido Mn(V) para generar el complejo Mn(VI).
- Cristalografía de rayos X para la determinación estructural.
- Reacciones con fosfinas, estirenos y análogos de NADH.
- Estudios de Hammett y mediciones del efecto del isótopo cinético.
- Espectrometría de masas de ionización por electrospray (ESI/MS) y espectroscopia de infrarrojos (IR).
Principales resultados:
- Aislamiento y caracterización estructural de rayos X de un complejo de nitrido Mn (VI) estable.
- Se ha demostrado la transferencia del átomo N a la trifenilfosfina y los estirenos, formando Ph3PNH y aziridinas.
- Comportamiento electrófilo y nucleófilo observado en reacciones con estirenos sustituidos (trama de Hammett en forma de V).
- Reacciones exitosas de transferencia de hidruro con análogos de NADH (AcrH2 y BNAH) con un efecto cinético isotópico de 7.3.
- Caracterización del producto [MnV(N) ((TAML-H+) ]
Conclusiones:
- El estudio aisló y caracterizó con éxito un complejo de nitrido de Mn (VI) raro y estable.
- El complejo exhibe una reactividad versátil, incluida la transferencia de átomos de N y la transferencia de hidritos.
- Las reacciones de transferencia de hidrógeno proceden a través de un mecanismo de "transferencia concertada de protones-electrones separados" (CPET), con el protón transferido al oxígeno carbonilo del ligando TAML.
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